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Unraveling the Impact of Halide Mixing on Perovskite Stability

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.8b11210· OSTI ID:1542287
 [1];  [2];  [1];  [1];  [1];  [3];  [1];  [4];  [2];  [1]
  1. Okinawa Inst. of Science and Technology Graduate Univ. (OIST), Onna-son, Okinawa (Japan). Energy Materials and Surface Sciences Unit (EMSSU)
  2. Univ. of Toledo, Toledo, OH (United States). Dept. of Physics and Astronomy and Wright Center for Photovoltaics Innovation and Commercialization
  3. Okinawa Inst. of Science and Technology Graduate Univ. (OIST), Onna-son, Okinawa (Japan). Energy Materials and Surface Sciences Unit (EMSSU); Univ. Siegen, Seigen (Germany). Dept. Physik
  4. CSIC and The Barcelona Inst. of Science and Technology, Barcelona (Spain). Catalan Inst. of Nanoscience and Nanotechnology (ICN2); Institució Catalana de Recerca i Estudis Avançats (ICREA), Barcelona (Spain)
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Increasing the stability of perovskites is essential for their integration in commercial photovoltaic devices. Halide mixing is suggested as a powerful strategy toward stable perovskite materials. However, the stabilizing effect of the halides critically depends on their distribution in the mixed compound, a topic that is currently under intense debate. In this paper, we successfully determine the exact location of the I and Cl anions in the CH3NH3PbBr3–yIy and CH3NH3PbBr3–zClz mixed halide perovskite lattices and correlate it with the enhanced stability we find for the latter. By combining scanning tunneling microscopy and density functional theory, we predict that, for low ratios, iodine and chlorine incorporation have different effects on the electronic properties and stability of the CH3NH3PbBr3 perovskite material. In addition, we determine the optimal Cl incorporation ratio for stability increase without detrimental band gap modification, providing an important direction for the fabrication of stable perovskite devices. The increased material stability induced by chlorine incorporation is verified by performing photoelectron spectroscopy on a half-cell device architecture. Our findings provide an answer to the current debate on halide incorporation and demonstrate their direct influence on device stability.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1542287
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 8 Vol. 141; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (8)

Unraveling the Impact of Halide Mixing on Crystallization and Phase Evolution in CsPbX3 Perovskite Solar Cells journal January 2021
Progress of Surface Science Studies on ABX 3 ‐Based Metal Halide Perovskite Solar Cells journal April 2020
Verringerung schädlicher Defekte für leistungsstarke Metallhalogenid‐Perowskit‐Solarzellen journal April 2020
Reducing Detrimental Defects for High‐Performance Metal Halide Perovskite Solar Cells journal January 2020
Ascorbic Acid‐Assisted Stabilization of α‐Phase CsPbI 3 Perovskite for Efficient and Stable Photovoltaic Devices journal August 2019
Effects of precursor composition on morphology and microstructure of hybrid organic–inorganic perovskite solar cells journal June 2019
Electronic structure of MAPbI3 and MAPbCl3: importance of band alignment journal October 2019
Polarization-enhanced photoelectric performance in a molecular ferroelectric hexane-1,6-diammonium pentaiodobismuth (HDA-BiI 5 )-based solar device journal January 2020

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